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Register a new userRovibrational cooling of molecules by optical pumping
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We demonstrate rotational and vibrational cooling of cesium dimers by optical pumping techniques. We use two laser sources exciting all the populated rovibrational states, except a target state that thus behaves like a dark state where molecules pile up thanks to absorption-spontaneous emission cycles. We are able to accumulate photoassociated cold Cs2 molecules in their absolute ground state (v = 0, J = 0) with up to 40% efficiency. Given its simplicity, the method could be extended to other molecules and molecular beams. It also opens up general perspectives in laser cooling the external degrees of freedom of molecules.
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Cooling the rotation and the vibration of molecules by broadband light sources was possible for trapped molecular ions or ultracold molecules. Because of a low power spectral density, the cooling timescale has never fell below than a few milliseconds. Here we report on rotational and vibrational cooling of a supersonic beam of barium monofluoride molecules in less than 440 $mu$s. Vibrational cooling was optimized by enhancing the spectral power density of a semiconductor light source at the underlying molecular transitions allowing us to transfer all the populations of $v=1-3$ into the vibrational ground state ($v=0$). Rotational cooling, that requires an efficient vibrational pumping, was then achieved. According to a Boltzmann fit, the rotation temperature was reduced by almost a factor of 10. In this fashion, the population of the lowest rotational levels increased by more than one order of magnitude.
We have recently demonstrated that optical pumping methods combined with photoassociation of ultra-cold atoms can produce ultra-cold and dense samples of molecules in their absolute rovibronic ground state. More generally, both the external and internal degrees of freedom can be cooled by addressing selected rovibrational levels on demand. Here, we recall the basic concepts and main steps of our experiments, including the excitation schemes and detection techniques we use to achieve the rovibrational cooling of Cs2 molecules. In addition, we present the determination of formation pathways and a theoretical analysis explaining the experimental observations. These simulations improves the spectroscopic knowledge required to transfer molecules to any desired rovibrational level.
We propose and experimentally investigate a scheme for narrow-line cooling of KRb molecules in the rovibrational ground state. We show that the spin-forbidden $mathrm{X^1Sigma^+} rightarrow mathrm{b^3Pi_{0^+}}$ transition of KRb is ideal for realizing narrow-line laser cooling of molecules because it has highly diagonal Franck-Condon factors and narrow linewidth. In order to confirm the prediction, we performed the optical and microwave spectroscopy of ultracold $^{41}$K$^{87}$Rb molecules, and determined the linewidth ($2pitimes$ 4.9(4) kHz) and Franck-Condon factors for the $mathrm{X^1Sigma^+} (v=0) rightarrow mathrm{b^3Pi_{0^+}} (v=0)$ transition (0.9474(1)). This result opens the door towards all-optical production of polar molecules at sub-microkelvin temperatures.
In this work we discuss the rotational structure of Rydberg molecules. We calculate the complete wave function in a laboratory fixed frame and derive the transition matrix elements for the pho- toassociation of free ground state atoms. We discuss the implications for the excitation of different rotational states as well as the shape of the angular nuclear wave function. We find a rather com- plex shape and unintuitive coupling strengths, depending on the angular momenta coupling that are relevant for the states. This work explains the different steps to calculate the wave functions and the transition matrix elements in a way, that they can be directly transferred to different molecular states, atomic species or molecular coupling cases.
We demonstrate the conversion of cold Cs_{2} molecules initially distributed over several vibrational levels of the lowest triplet state a^{3}Sigma_{u}^{+} into the singlet ground state X^{1}Sigma_{g}^{+}. This conversion is realized by a broadband laser exciting the molecules to a well-chosen state from which they may decay to the singlet state througtextcolor{black}{h two sequential single-photon emission steps: Th}e first photon populates levels with mixed triplet-singlet character, making possible a second spontaneous emission down to several vibrational levels of the X^{1}Sigma_{g}^{+} states. By adding an optical scheme for vibrational cooling, a substantial fraction of molecules are transferred to the ground vibrational level of the singlet state. The efficiency of the conversion process, with and without vibrational cooling, is discussed at the end of the article. The presented conversion is general in scope and could be extended to other molecules.
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